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At least 1,477 records · Page 82
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Co-occurrence of extremes in surface ozone, particulate matter, and temperature over eastern North America

Significance Exposure to extreme temperatures and high levels of the pollutants ozone and particulate matter poses a major threat to human health. Heat waves and pollution episodes share common underlying meteorological drivers and thus often coincide, which can synergistically worsen their health impacts beyond the sum of their individual effects. Furthermore, there is evidence that pollution episodes and heat waves will worsen under future climate change, making it imperative to understand the nature of their co-occurrence. In this paper, using 15 years of surface observations over the eastern United States and Canada, we show that the extremes cluster together in often overlapping large-scale episodes, and that the largest episodes have the hottest temperatures and highest levels of pollution.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Development of a standard capture efficiency test method for residential kitchen ventilation

Cooking activities are a major source of indoor air pollutants. To control pollutants generated from cooking activities, a range hood is commonly used in residential kitchens. Several building codes require that a range hood be installed in new homes to control pollutants from cooking, and the required airflow rates for range hoods are specified by indoor air quality standards. However, airflow alone does not show how much of the cooking pollutants are exhausted by the range hood. A better metric to evaluate range hood indoor air quality performance is capture efficiency -- the fraction of contaminants emitted during cooking that are exhausted directly to the outside via the range hood. The current article summarizes the development of a range hood capture efficiency test method for use in laboratory testing and equipment rating.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2022

Climate change penalty and benefit on surface ozone: a global perspective based on CMIP6 earth system models

Abstract This work presents an analysis of the effect of climate change on surface ozone discussing the related penalties and benefits around the globe from the global modelling perspective based on simulations with five CMIP6 (Coupled Model Intercomparison Project Phase 6) Earth System Models. As part of AerChemMIP (Aerosol Chemistry Model Intercomparison Project) all models conducted simulation experiments considering future climate (ssp370SST) and present-day climate (ssp370pdSST) under the same future emissions trajectory (SSP3-7.0). A multi-model global average climate change benefit on surface ozone of −0.96 ± 0.07 ppbv °C −1 is calculated which is mainly linked to the dominating role of enhanced ozone destruction with higher water vapour abundances under a warmer climate. Over regions remote from pollution sources, there is a robust decline in mean surface ozone concentration on an annual basis as well as for boreal winter and summer varying spatially from −0.2 to −2 ppbv °C −1 , with strongest decline over tropical oceanic regions. The implication is that over regions remote from pollution sources (except over the Arctic) there is a consistent climate change benefit for baseline ozone due to global warming. However, ozone increases over regions close to anthropogenic pollution sources or close to enhanced natural biogenic volatile organic compounds emission sources with a rate ranging regionally from 0.2 to 2 ppbv C −1 , implying a regional surface ozone penalty due to global warming. Overall, the future climate change enhances the efficiency of precursor emissions to generate surface ozone in polluted regions and thus the magnitude of this effect depends on the regional emission changes considered in this study within the SSP3_7.0 scenario. The comparison of the climate change impact effect on surface ozone versus the combined effect of climate and emission changes indicates the dominant role of precursor emission changes in projecting surface ozone concentrations under future climate change scenarios.

Zanis, Prodromos↗
DOE OSTI2022

Characterizing and quantifying uncertainty in projections of climate change impacts on air quality

Climate change can aggravate air pollution, with important public health and environmental consequences. While major sources of uncertainty in climate change projections - greenhouse gas (GHG) emissions scenario, model response, and internal variability - have been investigated extensively, their propagation to estimates of air quality impacts has not been systematically assessed. Here, we compare these uncertainties using a coupled modeling framework that includes a human activity model, an Earth system model of intermediate complexity, and a global atmospheric chemistry model. Uncertainties in projections of U.S. air quality under 21st century climate change are quantified based on a climate-chemistry ensemble that includes multiple initializations, representations of climate sensitivity, and climate policy scenarios, under constant air pollution emissions. We find that climate-related uncertainties are comparable at mid-century, making it difficult to distinguish the impact of variations in GHG emissions on ozone and particulate matter pollution. While GHG emissions scenario eventually becomes the dominant uncertainty based on the scenarios considered, all sources of uncertainty are significant through the end of the century. The results provide insights into intrinsically different uncertainties in projections of air pollution impacts and the potential for large ensembles to better capture them.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Subsurface landfill leachate contamination affects microbial metabolic potential and gene expression in the Banisveld aquifer

Microbial communities in groundwater ecosystems can develop the capacity to degrade complex mixtures of chemicals resulting from pollution by landfill leachate. Monitoring this natural attenuation requires insight into the metabolic potential and activity of microbial communities. We contrasted the metagenomes and metatranscriptomes from a leachate-polluted aquifer downstream of the Banisveld (the Netherlands) landfill with uncontaminated groundwater, which revealed changes in microbial genomic content and activity. Banisveld landfill leachate contains mono-aromatic hydrocarbons and the assessment of natural attenuation of these compounds in the aquifer had been a focal point of research. In the contaminated groundwater, active microbial functions were the ones involved in degradation of complex carbon substrates and organic pollutants. We found that benzylsuccinate synthase genes-involved in the catabolism of toluene-were highly expressed close to the source of contamination, confirming the ongoing natural attenuation of organic mono-aromatic hydrocarbon pollution in this aquifer. Additionally, metatranscriptomes were indicative of phosphorus limitation that can constrain total microbial activity and agree with the low phosphate concentrations (<0.4 μmol/L) in this aquifer. Through the application of metagenomics and metatranscriptomics, we were able to determine functional potential and expression patterns to assess the natural attenuation processes and constraints on microbial communities.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Location generalizability of image-based air quality models

This paper is to be submitted at the IEEE/CVF Winter Conference on Applications of Computer Vision (WACV) Computer Vision for Earth Observation workshop. The full paper abstract is below: The ability to rapidly quantify atmospheric pollutants is important both for global emissions monitoring and for mitigating the adverse effects that follow a hazardous chemical release. In the aftermath of a chemical release, imagery is often the only available resource to assess local conditions. Recent work has demonstrated initial success in predicting particulate matter pollution from imagery; however, these results are tied to a specific site and do not generalize to new geographic locations. In this work, we seek to understand how easily deep learning models generalize to new locations in the context of image-based air quality assessments, targeting two distinct tasks: (1) broad measures of particulate matter pollution, and (2) the mass of a given chemical released in hazardous plumes. For the latter, we focus on sulfur dioxide, a toxic aerosol and a major component of particulate matter pollution caused by industrial fossil fuel consumption. To develop a model that operates in the widest possible range of environments, we test different training strategies, including the use of new geolocation foundation models. The best performing models achieve >80% accuracy when evaluating unseen imagery at previously seen sites, but we find significant drops in performance when evaluating imagery from unseen sites, at best 65%. Additionally, we present the public release of the National Parks Air Quality Index Dataset, a new medium-sized dataset that pairs imagery with sensor-based air quality measurements at 15 different national parks.

Byler, Eleanor B. [BATTELLE (PACIFIC NW LAB)]↗
DOE OSTI2015

Quantify the energy and environmental benefits of implementing energy-efficiency measures in China’s iron and steel production

As one of the most energy-, emission- and pollution-intensive industries, iron and steel production is responsible for significant emissions of greenhouse gas (GHG) and air pollutants. Although many energy-efficiency measures have been proposed by the Chinese government to mitigate GHG emissions and to improve air quality, lacking full understanding of the costs and benefits has created barriers against implementing these measures widely. This paper sets out to advance the understanding by addressing the knowledge gap in costs, benefits, and cost-effectiveness of energy-efficiency measures in iron and steel production. Specifically, we build a new evaluation framework to quantify energy benefits and environmental benefits (i.e., CO 2 emission reduction, air-pollutants emission reduction and water savings) associated with 36 energy-efficiency measures. Results show that inclusion of benefits from CO 2 and air-pollutants emission reduction affects the cost-effectiveness of energy-efficiency measures significantly, while impacts from water-savings benefits are moderate but notable when compared to the effects by considering energy benefits alone. The new information resulted from this study should be used to augment future programs and efforts in reducing energy use and environmental impacts associated with steel production.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2017

Assessing Occupant and Outdoor Air Impacts on Indoor Air Quality in New California Homes

In 2008 the State of California adopted new building codes that required the use of mechanical ventilation systems in homes that meet the requirements of ASHRAE Standard 62.2. The standard requires both a dwelling unit mechanical ventilation system and exhaust fans in kitchens and bathrooms. A field study was undertaken to evaluate the IAQ and ventilation performance of homes built to these requirements. For ventilation system performance, the airflows of all mechanical ventilation systems were measured and their use was monitored for a one-week period. To evaluate IAQ, key pollutants were measured indoors and outdoors during the week, and occupants completed satisfaction surveys. The key pollutants included: formaldehyde, humidity, PM2.5 and NO2. Passive samplers were used to determine average concentrations for the week. Active samplers were used to develop time-series results that can be used to correlate pollutant concentrations with occupant activities. Other ventilation/IAQ related parameters were also recorded, such as stove top temperatures to indicate cooking, exterior door contact switches to know when large openings were being used for ventilation and sensors to determine when clothes dryers were being used. The building envelope and duct leakage were measured to enable estimates of infiltration and duct leakage effects. This paper presents an overview of the test procedures and preliminary results from several homes. The results show that although average concentrations may be reasonable compared to available standards (with the exception of formaldehyde), occupants have a strong impact on pollutant variability and source strength and that outdoor concentrations cannot be ignored. Overall, these mechanically ventilated homes have reasonable IAQ. The homes and duct systems are moderately tight, though not excessively so, by US standards. Significant concerns have been expressed regarding compliance with the ventilation requirements in the California building code. However, almost all the ventilation systems in this study complied with the ventilation air flow requirements and on average were significantly higher than the minimum required air flow rates.

Walker, IS↗
DOE OSTI2013

Effect Of Ventilation On Chronic Health Risks In Schools And Offices

This study provides a risk assessment for chronic health risks from inhalation exposure to indoor air pollutants in offices and schools with a focus how ventilation impacts exposures to, and risks from, volatile organic compounds (VOCs) and particulate matter (PM2.5). We estimate how much health risks could change with varying ventilation rates under two scenarios: (i) halving the measured ventilation rates and (ii) doubling the measured ventilation rates. For the hazard characterization we draw upon prior papers that identified pollutants potentially affecting health with indoor air concentrations responsive to changes in ventilation rates. For exposure assessment we determine representative concentrations of pollutants using data available in current literature and model changes in exposures with changes in ventilation rates. As a metric of disease burden, we use disability adjusted life years (DALYs) to address both cancer and non-cancer effects. We also compare exposures to guidelines published by regulatory agencies to assess chronic health risks. Chronic health risks are driven primarily by particulate matter exposure, with an estimated baseline disease burden of 150 DALYs per 100,000 people in offices and 140 DALYs per 100,000 people in schools. Study results show that PM2.5-related DALYs are not very sensitive to changes in ventilation rates. Filtration is more effective at controlling PM2.5 concentrations and health effects. Non-cancer health effects contribute only a small fraction of the overall chronic health burden of populations in offices and schools (<1 DALY per 100,000 people). Cancer health effects dominate the disease burden in schools (3 DALYs per 100,000) and offices (5 DALYs per 100,000), with formaldehyde being the primary risk driver. In spite of large uncertainties in toxicological data and dose-response modeling, our results support the finding that ventilation rate changes do not have significant impacts on estimated chronic disease burdens. Median estimates of DALYs are approximately doubled when the ventilation rates are halved and there is little reduction in health risks associated with doubling ventilation rates, but the very low baseline disease burden from the indoor exposures we considered makes this unremarkable. In exploring the full range of exposure concentrations, to find the fraction exceeding the Office of Environmental Health and Hazard Assessment’s (OEHHAs) chronic reference exposure levels (cRELs) and United States Environmental Protection Agency’s (USEPA) chronic reference dose (RfD) we found only minor shifts in exposure safety margins when ventilation was doubled or halved. We combined our exposure estimates with cancer potency factors published by OEHHA and USEPA to determine that the annual excess cancer risk per capita are below 1 in a million under all ventilation rate scenarios for individual pollutants. The results indicate that chronic health risks (cancer and non-cancer) associated with VOC and PM2.5 exposure in offices and schools are low and thus the chronic disease burden or health benefits of ventilation changes are likely to be well below both the level of detection by health surveillance studies and the level of regulatory thresholds.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2019

2018 Idaho National Laboratory Annual Report for Permit to Construct P-2015.0023

The U.S. Department of Energy (DOE) Idaho National Laboratory (INL) Site operates facilities with potential emissions criteria and hazardous air pollutants. This report documents the calendar year 2018 criteria and hazardous air pollutants emissions and has been prepared to comply with permit to construct (PTC) P-2015-0023, Condition 2.9 and Idaho Administrative Procedures Act (IDAPA) 58.01.01.178, Standard Contents of Permits Establishing a Facility Emissions Cap. IDAPA 58.01.01.178.04 requires that all permits establishing a FEC shall include sufficient reporting to assure compliance with the permit establishing the FEC. Total hazardous air pollutant (HAP) emissions for the year were 1.49 tons in aggregate and the maximum individual HAP was hydrochloric acid at 1.26 tons. Criteria pollutant emissions were 2.16 tons for sulfur dioxide, 35.6 tons for oxides of nitrogen, 11.6 tons of carbon monoxide, 3.51 tons of total particulate matter and 2.66 tons of VOCs.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2019

Development of a Standard Test Method for Reducing the Uncertainties in Measuring the Capture Efficiency of Range Hoods

Cooking activities are a major source of indoor air pollutants. To control pollutants generated from cooking activities, a range hood is commonly used in residential kitchens. Several building codes require that a range hood be installed in new homes to control pollutants from cooking, and the required airflow rates for range hoods are specified by indoor air quality (IAQ) standards. However, air flow alone does not tell us how much of the cooking pollutants are exhausted by the range hood. A better metric to evaluate range hood IAQ performance is capture efficiency (CE)—the fraction of contaminants emitted during cooking that are exhausted directly to the outside via the range hood. This paper summarizes the development of a range hood CE test method for use in laboratory testing and equipment rating.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2023

Experimental Characterization of Hydrocarbons and Nitrogen Oxides Production in a Heavy-Duty Diesel–Natural Gas Reactivity-Controlled Compression Ignition Engine

Reactivity-Controlled Compression Ignition (RCCI) combustion is considered one of the most promising Low-Temperature Combustion (LTC) concepts aimed at reducing greenhouse gases for the transportation and power generation sectors. Due to the spontaneous combustion of a lean, nearly homogeneous mixture of air and low-reactivity fuel (LRF), ignited through the direct injection of a small quantity of high-reactivity fuel (HRF), RCCI (dual-fuel) shows higher efficiency and lower pollutants compared to conventional diesel combustion (CDC) if run at very advanced injection timing. Even though a HRF is used, the use of advanced injection timing leads to high ignition delays, compared to CDC, and generates high cycle-to-cycle variability, limited operating range, and high pressure rise rates at high loads. This work presents an experimental analysis performed on a heavy-duty single-cylinder compression ignited engine in dual-fuel diesel–natural gas mode. The objective of the present work is to investigate and highlight the correlations between combustion behavior and pollutant emissions, especially unburned hydrocarbons (HC) and oxides of nitrogen (NOx). Based on the analysis of crank-resolved pollutants measurements performed through fast FID and fast NOx systems under different engine operating conditions, two correlations were found demonstrating a good accordance between pollutant production and combustion behavior: Net Cyclic Hydrocarbon emission—cyclic IMEP variations (R 2 = 0.86), and Cyclic NOx—maximum value of the Rate of Heat Released (R 2 = 0.82).

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2017

Concentration Variations in Particulate Matter in Seoul Associated with Asian Dust and Smog Episodes

In this study, particulate species were measured in April–May 2003 at two sites, one in the megacity of Seoul and the other in the Deokjeok Island to the west of Seoul, to examine the effects of long-range transport under the influence of prevailing westerlies. The effects of Asian dust were observed in April, and a severe smog episode occurred in late May. During May, all air pollutants showed negative correlations with wind speed at Seoul, particularly for NO 2 and CO, a large proportion of which result from vehicle emissions. SO 4 2– continued to increase in association with an inflow of air pollutants from China with heavy use of coal, with fluctuations depending on wind speed. The smog episode in late May occurred as emissions from Siberian forest fires were superimposed on pollutant inflows from China that had persisted since early May and local emissions accumulated under stagnant conditions. During the episode, Siberian forest fires increased K + while local emissions primarily from vehicles increased NO 3 – , OC, and EC. The effects of an inflow of air pollutants from the outside were significant at Deokjeok, with small local emissions, resulting in substantial increases in Ca 2+ during the Asian dust event and SO 4 2– during the smog episode, compared to those at Seoul. Because both sites were strongly influenced by the effects of long-range transport in May, PM 2.5 along with SO 4 2– and K + exhibited a strong correlation between Seoul and Deokjeok.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Rapid urbanization and economic development in East Asia in past decades has led to photochemical air pollution problems such as excess photochemical ozone and aerosol formation. Asian megacities such as Seoul, Tokyo, Shanghai, Guangzhou, and Beijing are surrounded by densely forested areas, and recent research has consistently demonstrated the importance of biogenic volatile organic compounds (VOCs) from vegetation in determining oxidation capacity in the suburban Asian megacity regions. Uncertainties in constraining tropospheric oxidation capacity, dominated by hydroxyl radical, undermine our ability to assess regional photochemical air pollution problems. We present an observational data set of CO, NO x , SO 2 , ozone, HONO, and VOCs (anthropogenic and biogenic) from Taehwa research forest (TRF) near the Seoul metropolitan area in early June 2012. The data show that TRF is influenced both by aged pollution and fresh biogenic volatile organic compound emissions. With the data set, we diagnose HO x (OH, HO 2 , and RO 2 ) distributions calculated using the University of Washington chemical box model (UWCM v2.1) with near-explicit VOC oxidation mechanisms from MCM v3.2 (Master Chemical Mechanism). Uncertainty from unconstrained HONO sources and radical recycling processes highlighted in recent studies is examined using multiple model simulations with different model constraints. The results suggest that (1) different model simulation scenarios cause systematic differences in HO x distributions, especially OH levels (up to 2.5 times), and (2) radical destruction (HO 2 + HO 2 or HO 2 + RO 2 ) could be more efficient than radical recycling (RO 2 + NO), especially in the afternoon. Implications of the uncertainties in radical chemistry are discussed with respect to ozone–VOC–NO x sensitivity and VOC oxidation product formation rates. Overall, the NO x limited regime is assessed except for the morning hours (8 a.m. to 12 p.m. local standard time), but the degree of sensitivity can significantly vary depending on the model scenarios. The model results also suggest that RO 2 levels are positively correlated with oxygenated VOCs (OVOCs) production that is not routinely constrained by observations. These unconstrained OVOCs can cause higher-than-expected OH loss rates (missing OH reactivity) and secondary organic aerosol formation. The series of modeling experiments constrained by observations strongly urge observational constraint of the radical pool to enable precise understanding of regional photochemical pollution problems in the East Asian megacity region.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Aerosol-induced changes in the vertical structure of precipitation: a perspective of TRMM precipitation radar

Our knowledge is still poor regarding the response of the precipitation vertical structure to aerosols, partly due to the ignorance of precipitation occurring at different spatial scales. A total of 6 years of collocated ground-based PM 10 and satellite-based (Tropical Rainfall Measuring Mission, TRMM) radar data, along with ERA-Interim reanalysis, are used in this study to investigate the aerosol effects on three localized rain regimes (shallow, stratiform, and convective rain) over the Pearl River Delta region of China. A subjective analysis method is proposed to discriminate between the localized and synoptic-scale precipitations based on weather composite charts where daily averaged wind field at 850 hPa is overlaid with the geopotential height at 500 hPa. In general, average rain rate tends to be greater under polluted conditions than under clean conditions. But such potential aerosol effects are regime dependent: as the atmosphere becomes slightly polluted (PM 10 ≤38 µg m -3 ), the top 1 % radar reflectivity (Z) for all regimes initially increases, followed by continued increases and weak decreases for convective and stratiform/shallow rain regimes, respectively. As the atmosphere becomes much more polluted, such regime dependences of aerosol effects are more significant. From a perspective of the vertical Z structure, comparisons between polluted conditions (days with the highest third of PM 10 concentration) and clean conditions (days with the lowest third of PM 10 concentration) show that the convective rain regime exhibits a deeper and stronger Z pattern, whereas a much shallower and weaker Z pattern is observed for stratiform and shallow precipitation regimes. In particular, the top height of the 30 dBZ rain echo increases by ~29 % (~1.27 km) for the convective regime, but decreases by ~10.8 % (~0.47 km) for the stratiform regime. However, no noticeable changes are observed for the shallow precipitation regime. Impacts of meteorological factors are further studied on both rain top height (RTH) and the center of gravity of Z, including vertical velocity, vertical wind shear, convection available potential energy, and vertically integrated moisture flux divergence (MFD). The possible invigoration effect on convective precipitation seems dependent on wind shear, in good agreement with previous findings. Overall, the observed dependence of the precipitation vertical structure on ground-based PM 10 supports the notion of aerosol invigoration or suppression effect on cold or warm rain and adds new insights into the nature of the complex interactions between aerosol and various localized precipitation regimes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels

Organic aerosol (OA) is a major component of tropospheric submicron aerosol that contributes to air pollution and causes adverse effects on human health. Chemical transport models have difficulties in reproducing the variability in OA concentrations in polluted areas, hindering understanding of the OA budget and sources. Herein, we apply both process-based and observation-constrained schemes to simulate OA in GEOS-Chem. Comprehensive data sets of surface OA, OA components, secondary organic aerosol (SOA) precursors, and oxidants were used for model–observation comparisons. The base models generally underestimate the SOA concentrations in China. In the revised schemes, updates were made on the emissions, volatility distributions, and SOA yields of semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) and additional nitrous acid sources. With all the model improvements, both the process-based and observation-constrained SOA schemes can reproduce the observed mass concentrations of SOA and show spatial and seasonal consistency with each other. Our best model simulations suggest that anthropogenic SVOCs and IVOCs are the dominant source of SOA, with a contribution of over 50% in most of China, which should be considered for pollution mitigation in the future. The residential sector may be the predominant source of SVOCs and IVOCs in winter, despite large uncertainty remaining in the emissions of IVOCs from the residential sector in northern China. The industry sector is also an important source of IVOCs, especially in summer. More SVOC and IVOC measurements are needed to constrain their emissions. Besides, the results highlight the sensitivity of SOA to hydroxyl radical (OH) levels in winter in polluted environments. The addition of nitrous acid sources can lead to over 30% greater SOA mass concentrations in winter in northern China. It is important to have good OH simulations in air quality models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

The diurnal susceptibility of subtropical clouds to aerosols

The diurnal susceptibility of clouds and their radiative properties to aerosols is examined during their Lagrangian transition from subtropical stratocumulus to shallow cumulus regimes. Using large-eddy simulations, we analyze the six-day evolution of an air mass along a 3800 km observed trajectory from the coast of Peru toward the equator. Pristine and polluted scenarios are simulated with forcing imposed from weather reanalysis. The polluted scenario exhibits stronger diurnal variations in cloud water, cloud fraction, and albedo, with enhanced nighttime entrainment and suppressed precipitation. The overall response of cloud properties and outgoing shortwave radiation to droplet number concentration follows a distinct diurnal pattern: strong positive cloud adjustments dominate at night and in the morning, while weak negative adjustments prevail in the afternoon. This cycle is driven by the competition between precipitation suppression, which enhances cloud water and coverage, and entrainment drying, which depletes them. In polluted conditions, enhanced entrainment leads to a deeper and more decoupled boundary layer that cannot be sustained by surface fluxes in the afternoon, resulting in negative cloud adjustments. The enhanced entrainment rate under polluted conditions is caused by the reduced sedimentation of cloud and precipitation water from the entrainment zone. While the Twomey effect dominates the diurnal average albedo response, the diurnal variation in the competing cloud adjustments lead to a near-neutral net susceptibility in the afternoon, highlighting the critical role of diurnally varying processes in aerosol-cloud interactions.

Geosciences↗
DOE OSTI2014

Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Rapid urbanization and economic development in East Asia in past decades has led to photochemical air pollution problems such as excess photochemical ozone and aerosol formation. Asian megacities such as Seoul, Tokyo, Shanghai, Gangzhou, and Beijing are surrounded by densely forested areas and recent research has consistently demonstrated the importance of biogenic volatile organic compounds from vegetation in determining oxidation capacity in the suburban Asian megacity regions. Uncertainties in constraining tropospheric oxidation capacity, dominated by hydroxyl radical concentrations, undermine our ability to assess regional photochemical air pollution problems. We present an observational dataset of CO, NOX, SO2, ozone, HONO, and VOCs (anthropogenic and biogenic) from Taehwa Research Forest (TRF) near the Seoul Metropolitan Area (SMA) in early June 2012. The data show that TRF is influenced both by aged pollution and fresh BVOC emissions. With the dataset, we diagnose HOx (OH, HO2, and RO2) distributions calculated with the University of Washington Chemical Box Model (UWCM v 2.1). Uncertainty from unconstrained HONO sources and radical recycling processes highlighted in recent studies is examined using multiple model simulations with different model constraints. The results suggest that 1) different model simulation scenarios cause systematic differences in HOX distributions especially OH levels (up to 2.5 times) and 2) radical destruction (HO2+HO2 or HO2+RO2) could be more efficient than radical recycling (HO2+NO) especially in the afternoon. Implications of the uncertainties in radical chemistry are discussed with respect to ozone-VOC-NOX sensitivity and oxidation product formation rates. Overall, the VOC limited regime in ozone photochemistry is predicted but the degree of sensitivity can significantly vary depending on the model scenarios. The model results also suggest that RO2 levels are positively correlated with OVOCs production that is not routinely constrained by observations. These unconstrained OVOCs can cause higher than expected OH loss rates (missing OH reactivity) and secondary organic aerosol formation. The series of modeling experiments constrained by observations strongly urge observational constraint of the radical pool to enable precise understanding of regional photochemical pollution problems in the East Asian megacity region.

Kim, Saewung↗